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Physical Review A

Formation and detection of ultracold ground-state polar molecules

Christopher Haimberger, Jan Kleinert, Mishkatul Bhattacharya, N. P. Bigelow

Published Aug 27, 2004• 159 citations
Publisher

Abstract

We report on the formation of translationally cold $\mathrm{NaCs}$ molecules starting from a laser-cooled atomic vapor of $\mathrm{Na}$ and $\mathrm{Cs}$ atoms. Colliding atoms are transferred into bound molecular states in a two-step photoactivated process in which the atoms are first photoassociated by trap photons into an excited state molecular complex and then allowed to decay into a bound molecular ground state. Time-of-flight measurements show a translational temperature $T=260\ifmmode\pm\else\textpm\fi{}130\phantom{\rule{0.3em}{0ex}}\ensuremath{\mu}\mathrm{K}$ that reflects the measured temperature of the initial atomic gas.

DOI
10.1103/physreva.70.021402

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We report on the formation of translationally cold NaCs\mathrm{NaCs}NaCs molecules starting from a laser-cooled atomic vapor of Na\mathrm{Na}Na and Cs\mathrm{Cs}Cs atoms. Colliding atoms are transferred into bound molecular states in a two-step photoactivated process in which the atoms are first photoassociated by trap photons into an excited state molecular complex and then allowed to decay into a bound molecular ground state. Time-of-flight measurements show a translational temperature T=260\ifmmode±\else\textpm\fi130\ensuremathμKT=260\ifmmode\pm\else\textpm\fi{}130\phantom{\rule{0.3em}{0ex}}\ensuremath{\mu}\mathrm{K}T=260\ifmmode±\else\textpm\fi130\ensuremathμK that reflects the measured temperature of the initial atomic gas.
We report on the formation of translationally cold Cs2 ground-state molecules through photoassociation of laser-cooled cesium atoms in a magneto-optical trap. The cold molecules are obtained after spontaneous decay of photoassociated molecules, and detected after pulsed-laser photoionization into Cs2+ ions. Photoassociation spectra of cesium attractive molecular states below the 6S1/2+6P3/2 dissociation limits are reported, obtained with both ion detection and trap-loss method. A temperature as low as 20−5+15 has been measured for the molecular cloud.
In contrast to atoms, laser cooling of molecules is very difficult because of the lack of a closed two-level scheme for population recycling. Molecular photoassociation of cold atoms has permitted the first observation of the formation of cold ground state Cs 2 molecules. In this scheme, two free cold atoms absorb one photon, to form an electronically excited molecule in a well-defined ro-vibrational state, which yields translationally cold molecules, after spontaneous decay, in their ground state or in their lowest triplet state.
We have performed photoassociative spectroscopy of cold Cs atoms in a vapor-cell magneto-optical trap, within $10{\mathrm{cm}}^{\ensuremath{-}1}$ below the dissociation limit 6s2S1/2+6p2P3/26s^{2}S_{1/2}+6p^{2}P_{3/2}6s2S1/2​+6p2P3/2​. Our detection method is based on pulsed-laser photoionization of Cs2{\mathrm{Cs}}_{2}Cs2​ molecules, selectively detected through a time-of-flight mass spectrometer. Temporal and spatial analysis of Cs2+{\mathrm{Cs}}_{2}^{+}Cs2+​ ions show for the first time the formation of translationally cold Cs2{\mathrm{Cs}}_{2}Cs2​ triplet ground state molecules, at a temperature $T\ensuremath{\sim}300\ensuremath{\mu}\mathrm{K}$.
In the molecular photoassociation process, two free cold atoms absorb one photon by a resonant way, to create an excited molecule in a well defined ro-vibrational state. The photoassociative spectroscopy of alkaline dimers yields accurate determinations for the long-range parts of molecular potential curves correlated to the first s + p asymptote. In contrast to atoms, laser cooling of molecules is very difficult because of the lack of a closed two-level scheme for recycling the population. The molecular photoassociation of cold atoms opens also a promising alternative for the formation of cold ground state molecules. Photoassociation of cold cesium atoms has permitted the first observation of translationally cold ground state molecules. The case of the cesium atom is very favorable because the 0 g - and 1 u purely long-range states below the dissociation limit 6s 1/2 +6p 3/2 present Condon points at intermediate distances. Such configurations offer rather efficient channels for the creation of singlet or triplet ground state Cs 2 molecules after spontaneous decay.
We have produced ultracold polar RbCs molecules via photoassociation starting from laser-cooled 85 Rb and 133 Cs atoms in a dual-species, forced dark magneto-optical trap. The formed electronically excited RbCs* molecules correlated to the Rb(5S 1/2 ) + Cs(6P 1/2 ) dissociation limit are observed by trap loss spectroscopy. Following the decay of these excited RbCs* molecules, the formed ground state molecules are directly ionized by a two-photon single-color pulse dye laser, which is a new ionization mechanism for ground state RbCs molecules and thence detected by time-of-flight mass spectroscopy.
We present a theoretical analysis of optical pathways for formation of cold ground-state (NaCa)+{(\mathrm{NaCa})}^{+}(NaCa)+ molecular ions via an intermediate state. The formation schemes are based on ab initio potential energy curves and transition dipole moments calculated using effective-core-potential methods of quantum chemistry. In the proposed approach, starting from a mixture of cold trapped Ca+{\mathrm{Ca}}^{+}Ca+ ions immersed into an ultracold gas of Na atoms, (NaCa)+{(\mathrm{NaCa})}^{+}(NaCa)+ molecular ions are photoassociated in the excited $E^{1}\mathrm{\ensuremath{\Sigma}}^{+}$ electronic state and allowed to spontaneously decay either to the ground electronic state or an intermediate state from which the population is transferred to the ground state via an additional optical excitation. By analyzing all possible pathways, we find that the efficiency of a two-photon scheme, via either the $B^{1}\mathrm{\ensuremath{\Sigma}}^{+}$ or $C^{1}\mathrm{\ensuremath{\Sigma}}^{+}$ potential, is sufficient to produce significant quantities of ground-state (NaCa)+{(\mathrm{NaCa})}^{+}(NaCa)+ molecular ions. A single-step process results in lower formation rates that would require either a high-density sample or a very intense photoassociation laser to be viable.